Process of binding and utilizing air-nitrogen.



A. SINDING-LARSEN. PROCESS OF BINDING AND UTILIZING AIR NITROGEN.

APPLICATION FILED MAY15,1911

1,031,477. Patented July 2, 1912.

605 lfefcr Scrulcr:

rrnn srATns'rENT OFFICE ALF SINDIIiIGJiARSEN, OF CHRISTIANIA, NORWAY, ASSIGNOR TO MESSRS. STORM BULL & 00., OF cfiRlsTIANIA, NOR'WAY.

PROCESS OF BINDING AND UTILIZING AIR-NITROGEN.

Specification of Letters Patent.

Patented July 2, 1912.

Application filed May 15, 1911. Serial No. 627,107.

To all whom it may concern: H

Be It known that I, ALF Smmnc-inusnn,

a subject of the King of Norway, residing at' f vide a process for binding and utilizing" the nitrogen of the air, and it consists in heat ing, in a suitable furnace, oxid materials which preferably consist principally of silica or titanic acid, said materials being of 'nat' ural or technical origin, and with said materials is heated an. adequate amount of a reducing agent in. the presence of halogen or sulfur, or of compounds that readilv g1 ve 'otl' halogen or sulfur (for instance SiCl ,Cf...

etc.) The oxid materials may also. be heated with a mixture or a compound oi a halogen and sulfur (for instance S. ,Cl, so that volatile or sublilnating compounds o'tsilicon or titanium and halogen or sulfur are formed.

These compounds are treated with nitri'igen at a suitably high temperature either name;

diately, or after having been completely or partly freed from the by-products ror instance GO) and from the residual raw niaterial. The nitrogen-i will. then replace the halogen or sulfur, which will, in a free state or in combination with other reagents tires cut (00, S, etc.) enter into the first part at the process.

As an example of how the process may be carried out I will describe how silicon-intro gen compounds of various nitrogen content may be produced by the use of quartz, sand, coke or charcoal and nitrogen, as rials. and chlorin as the necessary halogen. As above stated the process may he carried out as a direct or an indirect process. In the first case, a mixture of coke and quartz or sand is heated to about white heat in a blast furnace, which permits the introduction-of raw material a t the too and the t, king out of the product from the bottom, but being otlicrwiseclosed tight. Somewhat above the bottom of this furnace a mixture of nitrogen and chlorin first introduced, Tetrac'hiorid'ot silicon .t'ormed which then reacts With the excess of quartz raw mate- I and coke to form silicon trichlorid. At the high ten'iperaturc present this trichlorid will he acted upon by the nltrogcn, so that silicon nitrogen compounds are formed, thcn silicon tetrachlorid is again formed, and so on. part oi: the volatile silicon dhloriu i compounds is liable to escape, iTOgCtllQlf -with the carbon mouoxid which is form'cd, and which has to he removed. In order th keep these back, the current of carbon monoxid is conducted through a suitable cooler, where said volatile compounds will be condensed and tl'icrcupi'in led back to the vt'urnacc. This process is illustrated in the accompanying drawing in vertical section, in which- 1 designates anclcctrical resistance furnacc oi the shaft type, E2 the resistance placed in the central part of the furnace, 2- a revoluble drum arranged at the bottom of the furnace and provided with chambers 41, 5 and 6, any one of which may be so placed as ..to communicate with the interior of the in rnace.

7 designates an inlet for nitrogen and chtorin, and 8 the outlet for the volatile reaction products.

9 designates a cooler, and 12 a reaction chamber supplied with watch,

1.3 designates an electrolytic cell for the production of the chlorin necessary for the process.

Il.) designates a combustion chamber in which carbon monoxid is burned and 20, 21 are scrubbers in which the combustion gases from the chamber 10 are treated with lime to absorb the carbon dioxid of said gases. A mixture of quartz and carbon is introduced into the shaft furnace 1 from above, and on l'P'iiillt-Q the central part of the t'urnace i heated by means of the resistance 3. rhioriu introduced at the inlet: 7 reacts with the mixture of silica and carbon forming silicon cnlorid, which again reacts with the nitrogen introduced together with the rhlorin, and forms silicon nitrid and chlorin.

The reactions may be illustrated by the following equations:

The carbon monoxid combines with some of the chlorin, forming carbonyl chlorid, which together with the excess of carbon i'noncxid leaves the furnace at the outlet 8 and is conducted into the cooler 9 where The .to remove the gaseous substances contained able compounds formed therefrom are then part of the carbonyl chlorid is condensed l and flows through the pipe 10 back into the furnace at 11. The silicon nitrid formed is discharged by turning the drum 3 onethird revolution to the left, so that the empty chamber 5 is brought directly below the discharge opening of the furnace. The chamber 4, which contains the siliconnitrid, is thereby brought into. the position of the chamber (5, and a. current of nitrogenfrom a conduit 23 blown through the same so as in the discharged product and to cool this next one-third revolution of the drum 3.

The mixture of carbonyl chlorid and carbon monoxid is passed from the cooler 9 into the chamber 12, Where the carbonyl chloridis decomposed by water according to the following equation:

The hydrochloric acid formed flowsinto the electrolytic cell 13, where it is de'composed, and the chlorin formed passes through the gas meter 14 into the furnace at 7. The-carbon monoxid from the chamber 12- is blown through a gas meter 16 into the combustion chamber 19, which is supplied With air by a fan 17 through a'gas meter 18. The combustion products are treated with. lime in the scrubbers 20 and 21. to absorb carbon dioxid, so that the gas leaving the scrubber 21. mainly consists of nitrogen, which is led into the shaft furnace at 6 through the pipes 22, 23, drum 3, gas meter 24 and pipe 15.

It may be of advantage to maintain two different temperature zones in the furnace, one at a red heat and one at a white heat. The chlorin is in this case brought into the furnace at the red-hot zone and the nitrogen at the white-hot zone. The othel, or indirect method of carrying out my invention consists in leading only chlorin (optionally carbonyl chlorid or silicon tetrachlorid) into said furnace, which has otherwise the same charge as above-mentioned. The s-ili eon chlorin compounds escaping with the carbon monoxid will become liquefied and then are led into a separate furnace where they are treated with nitrogen at high temperature, and it may be in the presence of a suitable amount of reagents (such as CO, S, etc.) which are able to take up the. chlorin liberated and to readily give it' 'iofi again. The chlorin or the easily decomposagain led back into the first furnace, while the s licon-nitrogen compounds formed are kept back 111 filters or deposition chambers 1. The process of binding and utilizing atmospheric nitrogen, which consists in treating oxid materials, together with a reducing agent at a raised temperature with ubstances consisting of or containing elements capable of forming volatile compounds with the base of said oxid material and treating the obtained volatile compounds with nitrogen at a raised. temperature.

2. The process of binding and utilizing atmospheric nitrogen which consists in treating materials containing silica together with a reducing agent at a raised temperature with a substance consisting of or containing elements capable. of forming Vela-- tile compounds with silicon and treating the obtained volatile compounds with nitrogen at a raised temperature.

3. The process of binding and utilizing atmospheric nitrogen, which consists in treating oxid materials together with a reducing agent at a raised temperature with substances consisting of or containing elements capable of forming volatile compounds with the base of said oxid material, treating the obtained volatile compound with nitrogen at a raised temperature producing hereby nitrogen compounds and a product consisting of or containing the above named elements and using said product again in the first part of the process.

4'. The process of binding and utilizing atmospheric nitrogen which consists in treating oXid materials together with a reducing agent. at a raised temperature with substances containing or, consisting of elements capable of forming volatile compounds'with he base of said oXid material and treating the obtained volatile com pounds with nitrogen in the presence of carbon Il'lOllUXld or other. substances capablc of taking up the above named elements. In testimony that I chiim the foregoing as myinvention, I have signed my name in presence of two subscrilnng witnesses.

ALF SINDING-LARSEN. Witnesses MARTIN GUTTORMSEN. NANA Pnnnasoivl 

